Static Magnetic Susceptibility Research Articles

Low-temperature cluster spin glass transition in the single-domain NiCr2O4 nanoparticles

NiCr2O4 nanoparticles with average particle size ∼15 nm, a single-domain size maintains the bulk canted antiferromagnetic ground state, were synthesized by a microwave combustion method. The magnetic behavior was carefully investigated by static and dynamic magnetic susceptibility measurements. In addition to a spin-glass-like behavior below paramagnetic-ferrimagnetic transition at T C, the NiCr2O4 nanoparticles demonstrate a low-temperature cluster spin glass transition below the spin canting transition T S, which manifests itself as a magnetic anomaly peak around ∼12 K (at 100 Oe) in the zero-field cooled magnetization with a relatively stronger field dependence in a ‘de Almeida-Thouless’ line for spin glasses. The AC susceptibility analyses in different approaches demonstrate a larger relative peak temperature variation per frequency decade and a longer characteristic relaxation time in the order of 0.04 and 10−7 s, against 0.01 and 10−9 s for the high-temperature blocking, indicating the slow spin dynamics for the low-temperature cluster glassy phase. A field-temperature magnetic phase diagram is proposed for the single-domain NiCr2O4 nanoparticles.

Magnetic collective state formation upon tuning the interparticle interactions in ensembles of ultrafine ferrihydrite nanoparticles

The results of a study of the dynamic (alternating current magnetic susceptibility) and static magnetic properties, as well as 57Fe Mössbauer spectrometry and ferromagnetic resonance of two-line ferrihydrite nanoparticle systems with varying intensities of magnetic interparticle interactions are reported. The strength of the magnetic interparticle interactions has been tuned by coating (with various degrees of coating) the ferrihydrite particles (2–4 nm in size and an average size ∼2.7 nm) of the initial synthetic sample by arabinogalactan. Also, a biogenic ferrihydrite sample (an average particle size of 2-nm) with a natural organic coating was studied and it has the weakest magnetic interparticle interactions among of all the samples. Relaxation times of the particle’s magnetic moment were determined by the data of static and dynamic magnetic susceptibilities and from analysis of 57Fe Mössbauer spectrometry. Based on the temperature dependences of the relaxation times, it has been concluded that the predominantly collective processes of freezing of the particle magnetic moments occur under the action of the magnetic interparticle interactions. It is shown that an important role in these processes is played by a magnetic subsystem of the surface spins of the particles. The effect of the interplay between the surface spin and magnetic moment subsystems on the static magnetic properties (low-temperature magnetic hysteresis loops) and the parameters of the microwave absorption line under the magnetic resonance conditions is discussed.

Intensity and lifetime ratiometric luminescent thermometer based on a Tb(III) coordination polymer.

A three-dimensional terbium(III) coordination polymer of formula [Tb(bttb)0.5(2,5-pzdc)0.5]n (1) [H4bttb = 1,2,4,5-tetrakis(4'-carboxyphenyl)benzene and H2-2,5-pzdc = 2,5-pyrazinedicarboxylic acid] was obtained under hydrothermal conditions. The bttb4- tetraanion in 1 adopts the bridging and chelating-bridging pseudo-oxo coordination modes while the 2,5-pzdc2- dianion exhibits a rather unusual bis-bidentate bridging pseudo-oxo coordination mode, both ligands being responsible for the stiffness of the resulting 3D structure. Solid-state photoluminescent measurements illustrate that 1 exhibits remarkable green luminescence emission, the most intense band occurring in the region of 550 nm (5D4 → 7F5) with lifetimes at the millisecond scale. Thermometric performances of 1 reveal a maximum relative sensitivity (Sm) of 0.76% K-1 at 295 K (δT = 0.05 K), constituting a TbIII ratiometric solid luminescent thermometer over the physiological temperature range. Variable-temperature static (dc) magnetic susceptibility measurements for 1 in the temperature range 2.0-300 K show the expected behavior for the depopulation of the splitted mJ levels of the 7F7 ground state of the magnetically anisotropic terbium(III) ion plus a weak antiferromagnetic interaction through the carboxylate bridges. No significant out-of-phase magnetic susceptibility signals were observed for 1 in the temperature range 2.0-10.0 K, either in the absence or presence of a static dc magnetic field.

Kondo screening in a Majorana metal

Kondo impurities provide a nontrivial probe to unravel the character of the excitations of a quantum spin liquid. In the S = 1/2 Kitaev model on the honeycomb lattice, Kondo impurities embedded in the spin-liquid host can be screened by itinerant Majorana fermions via gauge-flux binding. Here, we report experimental signatures of metallic-like Kondo screening at intermediate temperatures in the Kitaev honeycomb material α-RuCl3 with dilute Cr3+ (S = 3/2) impurities. The static magnetic susceptibility, the muon Knight shift, and the muon spin-relaxation rate all feature logarithmic divergences, a hallmark of a metallic Kondo effect. Concurrently, the linear coefficient of the magnetic specific heat is large in the same temperature regime, indicating the presence of a host Majorana metal. This observation opens new avenues for exploring uncharted Kondo physics in insulating quantum magnets.

Synthesis, Structure, and Magnetic and Biological Properties of Copper(II) Complexes with 1,3,4-Thiadiazole Derivatives.

New coordination compounds of copper(II) with 2,5-bis(ethylthio)-1,3,4-thiadiazole (L1) and 2,5-bis(pyridylmethylthio)-1,3,4-thiadiazole (L2) with compositions Cu(L1)2Br2, Cu(L1)(C2N3)2, Cu(L2)Cl2, and Cu(L2)Br2 were prepared. The complexes were identified and studied by CHN analysis, infrared (IR) spectroscopy, powder X-Ray diffraction (XRD), and static magnetic susceptibility. The crystal structures of Cu(II) complexes with L1 were determined. The structures of the coordination core of complexes Cu(L2)Cl2 and Cu(L2)Br2 were determined by Extended X-ray absorption fine structure (EXAFS) spectroscopy. Magnetization measurements have revealed various magnetic states in the studied complexes, ranging from an almost ideal paramagnet in Cu(L1)2Br2 to alternating-exchange antiferromagnetic chains in Cu(L1)(C2N3)2, where double dicyanamide bridges provide an unusually strong exchange interaction (J1/kB ≈ -23.5 K; J2/kB ≈ -20.2 K) between Cu(II) ions. The cytotoxic activity of copper(II) complexes with L2 was estimated on the human cell lines of breast adenocarcinoma (MCF-7) and hepatocellular carcinoma (HepG2).

Dynamic magnetic properties of magnetosomes

Magnetosomes are found in magnetotactic bacteria, and consist of linear chains of tens of single-domain magnetic nanoparticles of (magnetite) or (greigite), enclosed in a lipid bilayer membrane. The particles are typically in the size range 30–, and are practically monodisperse. Harnessing the power of biomineralisation could lead to efficient strategies for synthesising semiflexible dipolar filaments, and the development of optimum materials for applications, including in biomedicine. Brownian dynamics simulations of noninteracting magnetosomes, containing ferromagnetic nanoparticles, have been used to determine static properties, and the dynamical response to a weak AC magnetic field. Results are presented for the radius of gyration , the static magnetic susceptibility , the dynamic magnetic susceptibility , and the effective Brownian rotation time , all as functions of N. The results are compared to theoretical predictions of the flexibility, susceptibility, and rotational dynamics of such magnetic filaments.

Influence of rotational disorder in C60 on electrical conductivity

The rotational order and disorder of C60 molecules in a lattice strongly modulates the density of states at the Fermi level and exerts a large influence on electrical transport. We report herein a study of this influence at high temperatures by employing microwave conductivity and static magnetic susceptibility as the observation probes, focusing on Na2CsC60. Microwave conductivity becomes 30% higher on going from a low-temperature (LT) orientationally ordered phase (space group: Pa-3) to a freely rotational high-temperature (HT) disordered phase (space group: Fm-3m). The density of states at the Fermi level, DEF, evaluated by static magnetic susceptibility measurements, increases from 15.1 states eV−1 C60−1 for the LT ordered phase to 17.4 states eV−1 C60−1 for the HT disordered phase. Both microwave conductivity and magnetic susceptibility show that Na2CsC60 maintains its macroscopic metallicity at least up to 673 K, although local probe NMR studies suggest electron localization in the disordered state at high temperatures. The rotational disorder greatly increases the scattering of conduction electrons. Different temperature evolutions of DEF(Na2CsC60) implied by NMR spectrometry and SQUID magnetometry are discussed.

The in- and out-of-plane magnetisation of highly underdoped YBa2Cu3O6+x single crystals

Previously we have shown how measurements of static magnetic susceptibility χc(T) of YBa2Cu3O6+x single crystals for magnetic fields applied along the c-axis, and χab(T) for fields in the ab-plane, can give useful information about their thermodynamic properties which are still being hotly debated. SQUID magnetometry above the superconducting (s/c) transition temperature Tc is used for larger crystals, while piezolever torque magnetometry gives χc(T)-χab(T) for tiny crystals. Here we present new data for more heavily under-doped crystals with hole concentrations per CuO2 plane, p =0.058 to 0.073. We again find that the T-dependent anisotropy well above Tc arises from the pseudogap and the g-factor anisotropy, while at lower T there are Gaussian s/c fluctuations with a strong cut-off. This is possibly a different region where neutron scattering studies give evidence for competition between incommensurate magnetic short-range order and superconductivity. We have studied crystals with three values of x, measuring χc(T) and χab(T) immediately after fixing x by quenching on to a copper block and again after allowing sufficient time at room temperature for the Cu-O chains to order. Thus, we report data for three pairs of underdoped (UD) crystals with Tc ranging from 13 to 36 K, namely UD13 and UD20, UD15 and UD30, UD23 and UD36. As found previously for polycrystalline samples, ordering the Cu-O chains increases Tc and substantially reduces the Curie term. These are isotropic, in contrast to the Pauli-like susceptibility from the CuO2 planes where there is g factor anisotropy, and this allows us to make a powerful novel analysis. At higher T, χc(T)- χab(T) varies as a + bT where the bT term arises from the pseudogap. At lower T, deviations from this behaviour are analysed in terms of 2D or 3D Gaussian s/c fluctuations to obtain in-plane coherence lengths and upper critical fields as T→0.

Photoresponsive Magnetic Relaxation Behavior of a Highly Stable π···π Interaction-Stacked Framework Based on a DyIII Single-Ion Magnet

Endowing lanthanide single-ion magnets (Ln-SIMs) with high stability and stimulus responsiveness is of significance for the practical applications of these novel magnetic materials, but still of challenge at present. Herein, we report on a highly stable and photoresponsive Ln-SIM system achieved by designing and synthesizing a π···π interaction-stacked framework based on DyIII-SIM (πOF-1). Its molecular formula is [Dy(thqa)] (H3thqa = tris[(8-hydroxyquinoline-2-yl)methylene]amino). Each of its C3-symmetric molecules consists of a thqa3– ligand and a DyIII ion, and it is linked to three neighbors by intermolecular π···π interactions, forming a supermolecular two-dimensional (2D) honeycombed topology. Such unique structure endows πOF-1 with not only air and thermal stability but also excellent chemical stability in different solvents, even in alkali solutions, including a 20 M NaOH aqueous solution. Dual magnetic relaxation behavior was observed in πOF-1. Magnetic dilution revealed that it is related to π···π-mediated intermolecular magnetic interactions. More significantly, both the static magnetic susceptibility and the dual-relaxation behavior of πOF-1 show response to photoirradiation, which could be ascribed to the photo-triggered intermolecular π → π* charge transfer (CT). So far as we know, πOF-1 could be the first Ln-SIM system possessing both a high stability and photoresponsiveness, and also the first photoresponsive Ln-SIM supermolecular system that does not rely on the single-crystal to single-crystal (SCSC) structural transformation. Its successful design and synthesis suggests that the introduction of π···π interactions can be a new strategy to fabricate stable and/or photoresponsive Ln-SIMs.

Spin Crossover and Thermochromism in Iron(II) Complexes with 2,6-Bis(1H-imidazol-2-yl)-4-methoxypyridine.

New iron(II) complexes with 2,6-bis(1H-imidazol-2-yl)-4-methoxypyridine (L) of the composition [FeL2]An∙mH2O (A = SO42-, n = 1, m = 2 (I); A = ReO4-, n = 2, m = 1 (II); A = Br-, n = 2, m = 2 (III)) have been synthesized and investigated. To determine the coordination ability of the ligand, a single crystal of a copper(II) complex of the composition [CuLCl2] (IV) was obtained and studied by X-ray technique. Compounds I-III were studied using methods of X-ray phase analysis, electron (diffuse reflection spectra), infrared and Mössbauer spectroscopy, static magnetic susceptibility. The study of the µeff(T) dependence showed that the 1A1 ↔ 5T2 spin crossover manifests itself in the compounds. The spin crossover is accompanied by thermochromism: there is a distinct color change orange ↔ red-violet.

Electron Correlation Effects in Paramagnetic Cobalt

We study the influence of Coulomb correlations on spectral and magnetic properties of fcc cobalt using a combination of density functional theory and dynamical mean-field theory. The computed uniform and local magnetic susceptibilities obey the Curie–Weiss law, which, as we demonstrate, occurs due to the partial formation of local magnetic moments. We find that the lifetime of these moments in cobalt is significantly less than in bcc iron, suggesting a more itinerant magnetism in cobalt. In contrast to the bcc iron, the obtained electron self-energies exhibit a quasiparticle shape with the quasiparticle mass enhancement factor m*/m ~ 1.8, corresponding to moderately correlated metal. Finally, our calculations reveal that the static magnetic susceptibility of cobalt is dominated by ferromagnetic correlations, as evidenced by its momentum dependence.

Exchange interaction for Mn acceptors in GaAs: Revealing its strong deformation dependence

In this paper we calculate exchange interaction constant between manganese ion inner electronic $d$-shell and GaAs valence band bounded hole using their microscopic multiparticle wave functions. We reveal its parametric dependence on crystal lattice deformations and find out that it could be about and even more than dozens percent when the strain tensor reaches values of $10^{-3} \div 10^{-2}$. This fact is in accordance with the previous hypothesis of deformation dependence of Mn acceptors in GaAs fine energy structure obtained from Raman spectroscopy, and we show that this dependence has the same magnitude. Also, we resolve here the problem of a substantial high temperature mismatch between well-developed theory and experimental data for the static magnetic susceptibility of Mn ions in GaAs. We show by numerical estimates and calculations that quite a strong parametric dependence of the exchange coupling value on GaAs lattice expansion determines the high temperature (above $50~$K) magnetic susceptibility reduction as well.

First-principles calculation of the frequency-dependent dipole polarizability of argon

In this work we report state-of-the-art theoretical calculations of the dipole polarizability of the argon atom. Frequency dependence of the polarizability is taken into account by means of the dispersion coefficients (Cauchy coefficients), which is sufficient for experimentally relevant wavelengths below the first resonant frequency. In the proposed theoretical framework, all known physical effects including the relativistic, quantum electrodynamics, finite nuclear mass, and finite nuclear size corrections are accounted for. We obtained ${\ensuremath{\alpha}}_{0}=11.0775(19)$ for the static polarizability and ${\ensuremath{\alpha}}_{2}=27.976(15)$ and ${\ensuremath{\alpha}}_{4}=95.02(11)$ for the second and fourth dispersion coefficients, respectively. The result obtained for the static polarizability agrees (within the estimated uncertainty) with the most recent experimental data [C. Gaiser and B. Fellmuth, Phys. Rev. Lett. 120, 123203 (2018)] but is less accurate. The dispersion coefficients determined in this work appear to be the most accurate in the literature, improving by more than an order of magnitude upon previous estimates. By combining the experimentally determined value of the static polarizability with the dispersion coefficients from our calculations, the polarizability of argon can be calculated with accuracy of around $10\phantom{\rule{0.16em}{0ex}}\mathrm{ppm}$ for wavelengths above roughly $450\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$. This result is important from the point of view of quantum metrology, especially for a new pressure standard based on thermophysical properties of gaseous argon. Additionally, in this work we calculate the static magnetic susceptibility of argon, which relates the refractive index of dilute argon gas with its pressure. While our results for this quantity are less accurate than in the case of the polarizability, they can provide, via the Lorenz-Lorentz formula, the best available theoretical estimate of the refractive index of argon.

Thermodynamics and the pairon model for cuprates

Two recent papers explore the idea of ``pairons'' (incoherent bound pairs above ${T}_{c}$) as a model for the pseudogap in cuprate high-${T}_{c}$ superconductors. From this model the authors calculate the resultant electronic specific heat and static magnetic susceptibility. At elevated temperature the pairons thermally unbind causing a broad peak in the specific heat, additional to the second-order peak at ${T}_{c}$ where the pairons coherently condense. With this unbinding the electronic entropy recovers to its bare quasiparticle linear-in-$T$ value. We show that this is inconsistent with the measured specific heat which reveals an entropy which never recovers to the highest temperature investigated (about 400 K). In the case of ${\mathrm{Bi}}_{2}{\mathrm{Sr}}_{2}{\mathrm{CaCu}}_{2}{\mathrm{O}}_{8}$ and ${\mathrm{La}}_{2\ensuremath{-}x}{\mathrm{Sr}}_{x}{\mathrm{CuO}}_{4}$ there is a broad peak above ${T}_{c}$ in the specific heat coefficient, $\ensuremath{\gamma}$, but this arises from the nearby van Hove singularity (vHs) which is more distant in the case of ${\mathrm{Y}}_{0.8}{\mathrm{Ca}}_{0.2}{\mathrm{Ba}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{y}$ and therefore not discernible. We propose a number of further critical tests. In the pairon model the BCS ratios are not satisfied until vanishingly near where superconductivity disappears in the heavily overdoped region whereas, experimentally, these mean-field ratios are sustained across the overdoped regime once the pseudogap has closed at critical doping.

Transition from Pauli paramagnetism to Curie-Weiss behavior in vanadium

We study electron correlations and their impact on magnetic properties of bcc vanadium by a combination of density functional and dynamical mean-field theory. The calculated uniform magnetic susceptibility {in bcc structure} is of Pauli type at low temperatures, while it obeys the Curie-Weiss law at higher temperatures. Thus, we qualitatively reproduce the experimental temperature dependence of magnetic susceptibility without introducing the martensitic phase transition. Our results for local spin-spin correlation function and local susceptibility reveal that the Curie-Weiss behavior appears due to partial formation of local magnetic moments, which originate from $t_{2g}$ states and occur due to local spin correlations caused by Hund's rule coupling. At the same time, the fermionic quasiparticles remain well-defined, while the formation of local moments is accompanied by a deviation from the Fermi-liquid behavior. In particular, the self-energy of the $t_{2g}$ states shows the non-analytic frequency dependence, which is a characteristic of the spin-freezing behavior, while the quasiparticle damping changes approximately linearly with temperature in the intermediate temperature range $200$--$700$~K. By analyzing the momentum dependence of static magnetic susceptibility, we find incommensurate magnetic correlations, which may provide a mechanism for unconventional superconductivity at low temperatures.

The influence of anisotropy on the microstructure and magnetic properties of dipolar nanoplatelet suspensions.

In recent years, there has been an increasing interest in magnetic nanoparticles with non-spherical shapes. This is largely due to their broad span of tuneable properties, which allow for tailoring of the colloidal properties by altering the magnetic anisometry or shape anisotropy of the nanoparticle. Although extensive research has gone into novel synthesis methods, the theoretical and analytical treatment of magnetic colloidal suspensions still predominantly focuses on spherical particles. This paper explores the microstructure and initial static magnetic susceptibility of systems of anisometric dipolar magnetic nanoplatelets in order to understand the applicability of dipolar sphere-based theories and models for such systems. We find that the microstructure as characterized by the particle distribution and magnetic clustering of platelets diverges significantly from that of spheres both quantitatively and qualitatively. We find lower initial static magnetic susceptibilities in nanoplatelet systems than in comparable suspensions of dipolar spheres. At lower values of the magnetic coupling constant, this can be accounted for by applying corrections to the volume fraction. However, this approach is less accurate for systems with stronger magnetic interactions. By providing predictions of and explanations for the observed effects, we aim to facilitate the use of magnetic nanoplatelet suspensions in the broad range of applications.

Investigation of solutions of iron(II) complexes with tris(pyrazol-1-yl)methane, possessing the spin-crossover phenomenon

Using methods of static magnetic susceptibility, UV and visible spectrometry and conductometry, dimethylformamide solution of iron(II) complex with tris(pyrazol-1-yl)methane (HC(pz)3) having the composition [Fe(HC(pz)3)2]ns2 (ns = 2-naphthalene sulfonate) has been studied. In solution, as in the solid state, this compound exhibits a spin crossover of 1A1 ↔ 5T2, while in solution it is shifted to a region of lower temperatures and is sharper. It is shown that at a given concentration of 2.5 × 10−4 mol/L at 298 K, the molar electrical conductivity for the [Fe(HC(pz)3)2]ns2 complex in dimethylformamide is Λ298k = 100 ± 2 Ohm−1cm2 mol−1. Solutions of the [Fe(HC(pz)3)2]ns2 complex in a polar aprotic solvent with high dielectric permittivity are characterized by a high degree of dissociation by the type of 1,1-charging electrolyte. The dependences of the logarithm of the electrical conductivity of the studied solutions as a function of the logarithm of concentration and of 1/T are linear. The values of the electrolyte dissociation constant, pK = 2.3, and the activation energy of the charge transfer process, Ea = 5815 J/mol, are calculated. It is shown that a change in the spin state of the central atom of the complex in solution does not lead to changes in the nature of electrical conductivity and does not change Ea.

High-Temperature Spin Crossover in Iron(II) Complexes with 2,6-Bis(1H-imidazol-2-yl)pyridine

Novel iron(II) coordination compounds containing a ligand 2,6-bis(1H-imidazol-2-yl)pyridine (L), having such a composition as [FeL2]SO4·0.5H2O, [FeL2]Br2·H2O, [FeL2](ReO4)2, [FeL2]B10H10∙H2O, [FeL2]B12H12∙1.5H2O had been synthesized and studied using UV-Vis (diffuse reflectance), infrared, extended X-ray absorption fine structure (EXAFS), and Mössbauer spectroscopy methods, as well as X-ray diffraction and static magnetic susceptibility methods. The analysis of the μeff(T) dependence in the temperature range of 80–600 K have shown that all the obtained complexes exhibit a high-temperature spin crossover 1A1 ↔ 5T2.

Study of Spin-Crossover in Iron(II) Complexes with 2,6-Bis(4,5-Dimethyl-1H-Imidazol-2-yl)Pyridine and closo-Borate Anions

New iron(II) coordination compounds with 2,6-bis(4,5-dimethyl-1H-imidazol-2-yl)pyridine (L) and closo-borate(2–) anions [FeL2]B10H10⋅2H2O and [FeL2]B12H12⋅H2O have been synthesized. The compounds have been identified and studied by CHN analysis, electron spectroscopy (diffuse reflection spectroscopy), IR, Mössbauer, and EXAFS spectroscopies, X-ray powder diffraction, and static magnetic susceptibility. The structures of the coordination knots of complexes [FeL2]B10H10⋅2H2O and [FeL2]B12H12⋅H2O has been obtained by modeling the EXAFS spectra. The ligand is coordinated by the iron(II) ion in a tridentate-cyclic manner by two nitrogen atoms of imidazole cycles and a nitrogen atom of pyridine to form the FeN6 coordination knot. The study of the temperature dependence of the magnetic susceptibility in the range of 80–500 K has showed that the high-temperature spin-crossover 1А1 ↔ 5Т2 manifests itself in the obtained compounds.

Novel Copper(II) Complexes with Dipinodiazafluorene Ligands: Synthesis, Structure, Magnetic and Catalytic Properties.

The reactions of CuX2 (X = Cl, Br) with dipinodiazafluorenes yielded four new complexes [CuX2L1]2 (X = Cl (1), Br (2), L1 = (1R,3R,8R,10R)-2,2,9,9-Tetramethyl-3,4,7,8,9,10-hexahydro-1H-1,3:8,10-dimethanocyclopenta [1,2-b:5,4-b’]diquinolin-12(2H)-one) and [(CuX2)2L2]n (X = Cl (3), Br (4), L2 = (1R,3R,8R,10R,1’R,3’R,8’R,10’R)-2,2,2’,2’,9,9,9’,9’-Octamethyl-1,1’,2,2’,3,3’,4,4’,7,7’,8,8’,9,9’,10,10’-hexadecahydro-1,3:1’,3’:8,10:8’,10’-tetramethano-12,12’-bi(cyclopenta [1,2-b:5,4-b’]diquinolinylidene). The complexes were characterized by IR and EPR spectroscopy, HR-ESI-MS and elemental analysis. The crystal structures of compounds 1, 2 and 4 were determined by X-ray diffraction (XRD) analysis. Complexes 1–2 have a monomeric structure, while complex 4 has a polymeric structure due to additional coordinating N,N sites in L2. All complexes contain a binuclear fragment {Cu2(μ-X)2×2} (X = Cl, Br) in their structures. Each copper atom has a distorted square-pyramidal coordination environment formed by two nitrogen atoms and three halogen atoms. The Cu-Nax distance is elongated compared to Cu-Neq. The EPR spectra of compounds 1–4 in CH3CN confirm their paramagnetic nature due to the d9 electronic configuration of the copper(II) ion. The magnetic properties of all compounds were studied by the method of static magnetic susceptibility. For complexes 1 and 2, the effective magnetic moments are µeff ≈ 1.87 and 1.83 µB (per each Cu2+ ion), respectively, in the temperature range 50–300 K, which are close to the theoretical spin value (1.73 µB). Ferromagnetic exchange interactions between Cu(II) ions inside {Cu2(μ-X)2X2} (X = Cl, Br) dimers (J/kB ≈ 25 and 31 K for 1 and 2, respectively) or between dimers (θ′ ≈ 0.30 and 0.47 K for 1 and 2, respectively) were found at low temperatures. For compounds 3 and 4, the magnetic susceptibility is well described by the Curie–Weiss law in the temperature range 1.77–300 K with µeff ≈ 1.72 and 1.70 µB for 3 and 4, respectively, and weak antiferromagnetic interactions (θ ≈ −0.4 K for 3 and −0.65 K for 4). Complexes 1–4 exhibit high catalytic activity in the oxidation of alkanes and alcohols with peroxides. The maximum yield of cyclohexane oxidation products reached 50% (complex 3). Based on the data on the study of regio- and bond-selectivity, it was concluded that hydroxyl radicals play a decisive role in the oxidation reaction. The initial products in reactions with alkanes are alkyl hydroperoxides.